SEPARATION AND PURIFICATION TECHNOLOGY
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2023
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IF 8.6
Minghui Liu,Yutong Zhao,Ming Tian,Kejia Liu,Guoping Hu,Jian Zhang,Tianyan Xue,Tao Qi,Hui Zhang
Platinum group metals (PGMs) are scarce critical materials, and recovering PGMs from spent automotive catalysts (SAC) is economically and ecologically important. However, dissolving the Fe-Si-PGMs alloy derived from SAC is challenging, impeding PGMs recovery. This study aims to develop a more sustainable, efficient, and scalable leaching scheme. We demonstrate efficient leaching of Fe-Si-PGMs alloy using a thermochemical combined with mechanochemical leaching method with a HCl + FeCl 3 + H 2 O 2 solution. Kinetics parameters studies optimize the leaching process. The main obstacles to leaching are the chemical inertness of the alloy and the SiO 2 encapsulation formed. Ultimately, efficient dissolution of 99 % Pd, 95 % Pt and 88 % Rh was achieved, increasing PGMs leaching by 17 % compared to single thermochemical leaching. Additionally, this work remedies the scalability limitations of mechanochemical leaching and provides valuable insights for PGMs recovery.
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Journal of Water Process Engineering
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2023
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IF 7
Lilan Huang,Haimei Chen,Jin Han,Haojie Chen,Jian Pan,Zihan Zhao,Zhichao Dong,Hailin Cong
Printing and dying wastewater has a pervasive problem afflicting people worldwide due to negative impacts on ecosystems and humans. Herein, Fe/Cu bimetallic catalyst/polyethersulfone (4A-Fe@Cu/PES) mixed matrix membrane (APMMM) with macropore and high porosity were developed as catalytic membrane reactor for reduction of congo red (CR) in flow-through reaction. The forced flow of the reactants through the membrane improved the mass transfer and intensified the contact between reactants and immobilized catalysts, allowing for efficient adsorption and catalysis. Furthermore, the CR adsorption by 4A-Fe@Cu would form catalytic microzones in the membrane, which was conducive to further improving the catalytic efficiency. As a result, the apparent activation energy of dynamic catalysis (21.1 kJ/mol) was significantly decreased compared with that of static catalysis (93.7 kJ/mol). Therefore, the dynamic processes exhibited more excellent adsorption and catalytic efficiency. In cross-flow circulation mode, the maximum CR adsorption capacity of APMMM-18 (doping amount of 4A-Fe@Cu is 18.0 wt%) was 199.5 mg/g 4A-Fe@Cu with a catalyst/CR mass ratio of 1/1.5 and initial CR concentration of 50 mg/L. For catalysis, the APMMM-18 could remove 99.8 % CR after 5 h with a catalyst/CR mass ratio of 1/1.5 and 1.9 mM of H 2 O 2 at pH 8. The catalytic membranes showed much higher performances than 4A-Fe@Cu particles even under lower H 2 O 2 conditions. The intrinsic CR adsorption and degradation ratio of one layer of APMMM-18 under dead-end filtration was also investigated. The combination of the Fenton catalyst with the membrane process accomplished the effective removal of CR.
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APPLIED CATALYSIS A-GENERAL
·
2023
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IF 5.5
Huifang Feng,Yitong Sun,Qiaozhen Xu,Hong Liu
Developing efficient photocatalyst to promote the conversion of CO 2 into value-added chemicals remains challenging. Here, novel NH 2 -MIL-101(Fe)@Bi 2 MoO 6 S-scheme heterojunctions were fabricated via a solvothermal method, in which Bi 2 MoO 6 (BMO) nanoparticles uniformly growing on the NH 2 -MIL-101(Fe) (NM101) octahedrons with intimate contact interface. The resultant heterojunctions revealed significantly enhanced activity for CO 2 photoreduction. The optimal performance was achieved when the content of BMO was 10 wt%, and the formation rate of CO reached 67.0 μmol·g −1 ·h −1 under visible light illumination (with apparent quantum efficiency of 0.09 % at 450 nm), which was 3.2-fold of individual NM101. The boosting activity benefited from the formation of S-scheme heterojunction at the NM101 @BMO interfaces, which facilitated the separation of photoinduced electron-hole pairs with strong redox ability at the interface. This S-scheme charge transfer mechanism was further validated by the in-situ XPS and fluorescence probe molecular experiment. Besides, the intermediates and preliminary mechanism of photoreaction were unraveled based on in-situ DRIFTS analysis. This work provides some novel insights for designing efficient S-scheme photocatalysts for CO 2 photoreduction.
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Catalysts
·
2023
·Vol. 13
·期 8
·1150
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IF 3.9
Xinying Chen,He Zhang,Shizhe Xu,Xiaoge Du,Kaida Zhang,Chun-Po Hu,Sihui Zhan,Xueyue Mi,Wen Da Oh,Xiao Hu,Ziyong Pan,Yueping Bao
In the current work, a novel Co-Fe bimetallic immobilized cellulose hydrogel bead (CoFeO@CHB) was prepared via in situ chemical precipitation followed by heat treatment and applied for tetracycline (TC) degradation in the presence of peroxymonosulfate (PMS). The characterization results indicated that the Co-Fe particles were evenly distributed within the porous cellulose hydrogel beads, without affecting their morphologies or crystal structures. During the TC degradation, the CoFeO@CHB/PMS system showed a high resistance and stability to different water bodies, and the common anions and natural organic matters showed a limited effect on TC degradation. The chemical quenching experiments (using chemicals to react with specific reactive species) as well as electron paramagnetic resonance (EPR) results showed that CoFeO@CHB can effectively active PMS to generate multiple reactive oxygen species (ROS, such as SO4•−,•OH and1O2), in which the1O2-dominated non-radical pathway played a vital role in TC degradation. Both Co and Fe were proposed as the active sites for PMS activation, and the CoFeO@CHB/PMS system showed a high potential in practical application due to its high selectivity and robustness with much less toxic intermediate products. Furthermore, a long-term continuous home-made dead-end filtration device was constructed to evaluate the stability and application potential of the CoFeO@CHB/PMS system, in which a >70% removal was maintained in a continuous 800 min filtration. These results showed the promising potential for cellulose hydrogel beads utilized as a metal-based nanomaterial substrate for organic degradation via PMS activation.Keywords:hydrogels;peroxymonosulfate;non-radical;tetracycline
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INORGANIC CHEMISTRY
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2023
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IF 4.6
Shaokang Su,Wei Zhang,Ying Xie,Lihong Qi,Song Wang,Limin An,Kai Pan
Cobalt phosphide has been widely used in various catalytic reactions due to its excellent catalytic activity and stability. In contrast to the conventional synthesis of Co2P nanorods using expensive and toxic trioctylphosphine (TOP), this study employs a dual-ligand strategy to prepare iron-atom-doped monodisperse Co2P nanorods. The strategy involves the use of triphenylphosphite (TPOP) as a cost-effective and relatively less toxic strong ligand, alongside hexadecylamine (HDA) as a weaker ligand. The resultant atom-doped Co2P nanorods exhibited a large aspect ratio, providing a plentiful supply of active sites for electrocatalytic hydrogen evolution. In both alkaline and acidic electrolytes, achieving a current density of 10 mA cm–2 required overpotentials of 91 and 141 mV, respectively, with the optimal Co:Fe molar ratio of 1:0.2. The introduction of Fe atoms through doping increased the electron density at the Co atom sites, thereby enhancing H adsorption. This research offers a cost-effective and relatively low-toxicity method for the controlled fabrication of monodisperse transition-metal phosphide nanorods, enabling efficient catalytic reactions.
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CHEMICAL ENGINEERING JOURNAL
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2023
·
IF 15.1
Fangchao Cui,Lanling Li,Dangfeng Wang,Likun Ren,Jiesen Li,YiLin Lu,Yuqiong Meng,Rui Ma,Shulin Wang,Xuepeng Li,Tingting Li,Jianrong Li
Bacterial biofilm infections cause about 600 million foodborne illnesses and about 420,000 confirmed deaths annually. However, traditional antibiotics and emerging nanomaterials have the problem of causing bacterial resistance, no catalytic activity and low biocompatibility. Herein, one new antibacterial carbon dots-based nanozyme Fe/N-CDs was developed with antibiofilm ability, excellent peroxidase activity and high biocompatibility. The Fe/N-CDs nanozyme manifested outstanding broad-spectrum antibacterial activity (even multidrug-resistant bacteria) by catalyzing the decomposition of H 2 O 2 to •OH through a peroxide-like reaction (V max /K m =1.07×10 -6 /s), which was 5.35-fold that of horseradish peroxidase (V max /K m =0.20×10 -6 /s). The antibacterial activity increased more than 500-fold after catalysis. The inhibitory capability of Fe/N-CDs nanozyme for Hafinia alvei biofilm was up to 80.2% of by inhibiting extracellular polymeric substances, total protein, AKP enzyme and ATPase. Notably, no obvious cytotoxicity and development of bacteria resistance were observed after co-culturing with the Fe/N-CDs nanozyme. Furthermore, the fresh test results demonstrated that the Fe/N-CDs nanozyme could effectively extend the shelf life of salmon for 3–6 days. These findings indicated that nanozyme could be used to extend the shelf life of food. What’s more, this antibiofilm Fe/N-CDs nanozyme provides the potential idea for developing carbon-based nanomaterials with catalytic activity and prevention of bacterial infections in food preservation.
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CERAMICS INTERNATIONAL
·
2023
·
IF 5.2
Gang Li,Ruiyang Tan,Xiangcheng Lu,Xinyu Zhang,Chengcheng Zhang,Bohong Gao,Yuting Zhou,Ke Chen,Ping Chen,Xinyi Wang
Chemical composition and morphological optimization are both effective strategies for constructing excellent electromagnetic wave absorption (EMWA) materials. While efficient EMWA materials derived from both metal-organic frameworks (MOFs) and MXenes have been extensively studied, composites derived from the Hofmann framework with MXene have not been reported. In this study, we employed a Hofmann framework ([Fe(pz)Ni(CN) 4 ], pz = pyrazine) and MXene (Ti 3 C 2 T x ) to create new MXene@Hofmann (MH1 and MH2) composites, using a simple co-precipitation method with two different contents of [Fe(pz)Ni(CN) 4 ]. The FeNi/C/TiO 2 composites with a multi-layered structure inherited from MXene were prepared by annealing the MXene@Hofmann composites at 500, 600, and 700 °C, resulting in the formation of MH1-500/600/700 and MH2-500/600/700 composites. Their compositions, morphologies, electromagnetic parameters, and EMWA performances were characterized. For the composites with a high [Fe(pz)Ni(CN) 4 ] content, MH2-600 has a minimum reflection loss ( RL min ) value of −30.63 dB at a thickness of only 1.8 mm and the broadest effective absorption bandwidth (EAB) of 3.90 GHz at 2.0 mm, while MH2-700 exhibits superior EMWA performance with an RL min value of −34.34 dB at 1.9 mm and an EAB value of 4.96 GHz at 2.1 mm. Their impressive EMWA performance might be attributed to the synergistic dielectric loss and magnetic loss and also the impedance matching from the reasonable ratio of the magnetic and dielectric components. This work demonstrates an effective strategy for constructing EMWA materials from the Hofmann framework and MXene.
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ELECTROCHIMICA ACTA
·
2023
·
IF 6.6
Zhiwen Xu,Guangyu Chen,Fei Yang,Juhee Jang,Guimei Liu,Fei Xiao,Yan Sun,Xiaoyi Qiu,Weiwei Chen,Dong Su,Meng Gu,Minhua Shao
The development of inexpensive and high-performance bifunctional electrocatalysts for oxygen reduction reaction (ORR) and oxygen evolution reaction (OER) is of crucial significance for rechargeable metal-air batteries , but remains challenging. Herein, we report an ingenious bifunctional oxygen electrocatalyst integrating ZIF-derived carbon-anchored Fe/Ni single atoms, FeNi alloy nanoparticles , and graphene support (denoted as Fe/Ni-NC||FeNi@G). Synergizing highly active Fe single atoms for the ORR and highly efficient FeNi alloy nanoparticles for the OER, the as-constructed Fe/Ni-NC||FeNi@G catalyst exhibits outstanding bifunctionality; the potential gap between the OER potential at 10 mA cm –2 and the ORR half-wave potential is only 0.618 V, outperforming the benchmark Pt/C + Ir/C catalyst and most transition metal-based bifunctional catalysts reported in the literature. More importantly, the Fe/Ni-NC||FeNi@G-driven zinc-air battery (ZAB) delivers a maximum power density of ∼200 mW cm –2 , a specific capacity of 876 mAh g –1 , and excellent cycling stability with negligible voltage decay up to 500 hours (3000 cycles). This work provides an effective approach to designing highly efficient non-noble metal multifunctional catalysts for practical applications in rechargeable metal-air batteries.
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Catalysts
·
2023
·Vol. 13
·期 6
·924
·
IF 3.9
Li Xu,Yuxuan Dong,Wei Xu,Wen Zhang
Preparing high-performance electrocatalysts for oxygen evolution reaction (OER)s with high durability for seawater electrolysis is of great significance. Herein, reported a one-step solution-immersion synthesis strategy to prepare a (Ni/Fe/Mo)OOH catalyst on a nickel foam substrate that can be accomplished in 5 min under ambient temperature and pressure. The unique cluster morphology of the catalyst on the surface of electrodes effectively increases the number of active sites, and the presence of Mo, Ni, and Fe in the catalyst enhances the activity of the OER. In the electrolyte solution (1 mol/L NaOH), the electrode exhibited low OER overpotentials of 265 mV, 286 mV, and 332 mV at currents of 100 mA·cm−2, 400 mA·cm−2, and 1000 mA·cm−2, respectively. This electrode also demonstrated excellent performance in seawater splitting, and the overpotentials at currents of 100 mA·cm−2, 400 mA·cm−2, and 1000 mA·cm−2in alkaline seawater environments were 330 mV, 416 mV, and 514 mV, respectively. In the 72 h durability test, the voltage increase was within 10 mV, exhibiting the excellent durability of the (Ni/Fe/Mo)OOH electrocatalyst. Therefore, the electrode developed here shows potential in the application of seawater electrolysis for hydrogen generation.Keywords:oxygen evolution reaction;(Ni/Fe/Mo)OOH catalyst;ultrafast and facile synthesis;alkaline seawater electrolysis
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JOURNAL OF COLLOID AND INTERFACE SCIENCE
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2023
·
IF 9.9
Qun Ding,Xuejun Zou,Jun Ke,Yuying Dong,Yubo Cui,Hongchao Ma
Herein, a ternary TiO 2 /MIL-88A(Fe)/g-C 3 N 4 heterojunction is successfully constructed through a facile hydrothermal strategy for enhancing solar energy harvesting and efficiency of catalytic nitrogen reduction induced by enlarged light absorption range, increasing interfacial charge transfer ability and desirable stability. Under the simulated sunlight irradiation, the N 2 fixation experiment shows that the yield of NH 3 reaches 1084.31 μmol/(g·h) over the TiO 2 /MIL-88A(Fe)/g-C 3 N 4 photocatalyst, and the yield is significantly enhanced, which is 33.68 and 13.94 times that is higher than the pure TiO 2 and g-C 3 N 4 , respectively. In a mean time, the excellent performance of the photocatalytic N 2 fixation over the ternary TiO 2 /MIL-88A(Fe)/g-C 3 N 4 is verified based on density function theory calculation and the decisive step over the composite is investigated by calculating Gibbs free energies of nitrogen reduction paths. The performance enhancement mechanism of TiO 2 /MIL-88A(Fe)/g-C 3 N 4 is speculated, which indicates that the hybridized three-component system presents a desirable Z-scheme band alignment, resulting in the improvement of separation and transfer efficiency of photoinduced charge carriers. The article shows a new and high-efficiency TiO 2 /MIL-88A(Fe)/g-C 3 N 4 photocatalysis for excellent nitrogen reduction ability.
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International Journal of Electrochemical Science
·
2023
·
IF 1.5
Jun Chen,Boding Zhang,Bingxing Wang,Chengxing Cui,Songlin Wang,Jichao Wang,Wenlong Zhang
With high toxicity, carcinogenicity and teratogenicity, quinoline has been threatening human health and ecological environment. Herein, Fe-Co-Ni-P/g-C 3 N 4 particles are developed as electrochemical reactors to form a three-dimensional catalytic particle electrode system (3D-CPE) for efficient removal of quinoline from wastewater by electro-Fenton (EF) oxidation process. with reaction time of 30 min, the particles dosage of 50 g/L, pH of 3, conductivity of 11.5 ms/cm, and current density of 37.04 mA/cm 2 , the chemical oxygen demand (COD) removal rate can up to 90.95%. In addition, electron paramagnetic response (EPR) and radical scavenging tests are performed to determine the hydroxyl radicals of electrochemical processes produced. The degradation products are analyzed by high performance liquid chromatography-mass spectrometry (HPLC-MS). Finally, through theoretical calculation and analysis of degradation products, a reasonable degradation mechanism is proposed.
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CHEMOSPHERE
·
2023
·
IF 8.8
Yingqian Zhang,Zhifei Ma,Xianchuan Xie,Daishe Wu,Xing Peng,Jianlong Li
Zero-valent iron (ZVI) is a promising technology for groundwater treatment , and its efficiency primarily depends on the electron transfer . However, there are still some problems such as low electron efficiency of ZVI particles and high yield of iron sludge that limits the performance, which warrant further investigation. In our study, a silicotungsten acidified ZVI composite (m-WZVI) was synthesized by ball milling to activate PS to degrade phenol. m-WZVI has a better performance on phenol degradation (with a removal rate of 91.82%) than ball mill ZVI(m-ZVI) with persulfate (PS) (with a removal rate of 59.37%). Compared with m-ZVI, the first-order kinetic constant (k obs ) of m-WZVI/PS is 2–3 times higher than that of the others. Iron ion was gradually leached in m-WZVI/PS system, being only 2.11 mg/L after 30 min, having to avoid excessive consumption of active substances. The underlying mechanisms of m-WZVI for PS activation mainly include: 1) were elucidated through different characterizations analyses that accounted for silictungstic acid (STA) can be combined with ZVI, and a new electron donor (SiW 12 4− ) was obtained, which improved the transfer rate performance of electrons for activating PS; 2) singlet oxygen ( 1 O 2 ) is the main active substance for phenol degradation, but other radicals also played an important role. Therefore, m-WZVI has good prospects for improving the electron utilization of ZVI.
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